材料科学
兴奋剂
电荷(物理)
分析化学(期刊)
光合作用
原子物理学
物理
光电子学
环境化学
粒子物理学
化学
生物化学
作者
Xize Lu,Zongwei Chen,Zhuofeng Hu,Fuyu Liu,Zhihong Zuo,Zixiang Gao,Haiguang Zhang,Youcai Zhu,Runzeng Liu,Yongguang Yin,Yong Cai,Dongling Ma,Qingzhe Zhang
标识
DOI:10.1002/aenm.202401873
摘要
Abstract Photocatalytic oxygen reduction reaction (ORR) is an environmentally friendly and cost‐effective approach for H 2 O 2 synthesis. However, the current photosynthesis system suffers from sluggish kinetics, rapid recombination of photoexcited charge carriers, and weak redox potentials, resulting in unsatisfactory solar‐to‐chemical conversion efficiency. Herein, a Z‐scheme heterojunction (UiO/IKCN) is constructed through coupling I − /K + co‐doped g‐C 3 N 4 (IKCN) with NH 2 ‐UiO‐66, a typical metal‐organic framework material. Under visible light irradiation, the optimal UiO/IKCN exhibits exceptional H 2 O 2 production rates in pure water (13.3 mM g −1 h −1 ) and in isopropanol solution (72.6 mM g −1 h −1 ), that is 48.4 times higher than pristine CN in isopropanol (1.5 mM g −1 h −1 ). A high apparent quantum yield of 10.28% at 420 nm is achieved by UiO/IKCN, surpassing most previously reported values. The dominating role of two‐electron ORR in H 2 O 2 photosynthesis is elucidated in detail. The significantly enhanced photocatalytic activity can be attributed to the facilitated charge separation and Z‐scheme charge transfer, which are unambiguously verified by stable‐state surface photovoltage, transient photoluminescence, femtosecond transient absorption spectroscopy, in‐situ irradiated X‐ray photoelectron spectroscopy, and density functional theory calculations. This study represents the first exploration of H 2 O 2 production using NH 2 ‐UiO‐66 and provides insights into the rational design of Z‐scheme heterojunction for highly efficient photosynthesis.
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